We study the convection and mixing of CO 2 in a brine aquifer, where the spread of dissolved CO 2 is enhanced because of geochemical reactions with the host formations (calcite and dolomite), in addition to the extensively studied, buoyancy-driven mixing. The nonlinear convection is investigated under the assumptions of instantaneous chemical equilibrium, and that the dissipation of carbonate rocks solely depends on flow and transport and chemical speciation depends only on the equilibrium thermodynamics of the chemical system. The extent of convection is quantified in term of the CO 2 saturation volume of the storage formation. Our results suggest that the density increase of resident species causes significant enhancement in CO 2 dissolution, although no significant porosity and permeability alterations are observed. Furthermore, early saturation of the reservoir can have negative impact on CO 2 sequestration.

@article{osti_1257782,
title = {Reactive transport modeling of the enhancement of density-driven CO2 convective mixing in carbonate aquifers and its potential implication on geological carbon sequestration},
author = {Islam, Akand and Sun, Alexander Y. and Yang, Changbing},
abstractNote = {We study the convection and mixing of CO2 in a brine aquifer, where the spread of dissolved CO2 is enhanced because of geochemical reactions with the host formations (calcite and dolomite), in addition to the extensively studied, buoyancy-driven mixing. The nonlinear convection is investigated under the assumptions of instantaneous chemical equilibrium, and that the dissipation of carbonate rocks solely depends on flow and transport and chemical speciation depends only on the equilibrium thermodynamics of the chemical system. The extent of convection is quantified in term of the CO2 saturation volume of the storage formation. Our results suggest that the density increase of resident species causes significant enhancement in CO2 dissolution, although no significant porosity and permeability alterations are observed. Furthermore, early saturation of the reservoir can have negative impact on CO2 sequestration.},
doi = {10.1038/srep24768},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {2016},
month = {4}
}

In spite of the numerous studies on changes within the reservoir following CO 2 injection and the effects of CO 2 release into overlying aquifers, little or no literature is available on the effect of CO 2 release on rock between the storage reservoirs and subsurface. This is important, because the interactions that occur in this zone between the CO 2 storage reservoir and the subsurface may have a significant impact on risk analysis for CO 2 storage projects. To address this knowledge gap, relevant rock materials, temperatures and pressures were used to study mineralogical and elemental changes in thismore » intermediate zone. Furthermore, after rocks reacted with CO 2-acidified 0.01 M NaCl, liquid analysis showed an increase of major elements (e.g., Ca and Mg) and variable concentrations of potential contaminants (e.g., Sr and Ba); lower aqueous concentrations of these elements were observed in N 2 control experiments, likely due to differences in pH between the CO 2 and N 2 experiments. In experiments with As/Cd and/or organic spikes, representing potential contaminants in the CO 2 plume originating in the storage reservoir, most or all of these contaminants were removed from the aqueous phase. SEM and Mössbauer spectroscopy results showed the formation of new minerals and Fe oxides in some CO 2-reacted samples, indicating potential for contaminant removal through mineral incorporation or adsorption onto Fe oxides. These experiments show the interactions between the CO 2-laden plume and the rock between storage reservoirs and overlying aquifers have the potential to affect the level of risk to overlying groundwater, and should be considered during site selection and risk evaluation.« less

This paper presents a quantitative method to evaluate CO 2 concentration ([CO 2]) and stable carbon isotope ratio (δ 13C) as indicators for leakage detection at a geological carbon sequestration site by combining use of field release tests and a numerical modeling approach. A numerical model was developed to simulate CO 2 dynamics by considering diffusion, dissolution in soil water, and soil respiration. The numerical model fits the background dynamics of [CO 2] (360 to 550 ppm) and δ 13C (-16‰ to -6‰) well and reproduces fairly the overall trend observed during the CO 2 release test. The model wasmore » further applied to assess detection probability (DP) of [CO 2] and δ 13C for leakage detection in terms of various factors, such as CO 2 leakage rate, background variations, δ 13C of the CO 2 leaked, and the threshold value of signal-to-noise ratio. Modeling results suggest that δ 13C may have a higher DP than [CO 2]. This study also shows that DP of δ 13C for the IEA Weyburn project is close to 0, implying δ 13C is inappropriate to be an indicator for CO 2 leakage at the site. Finally, the quantitative method developed can also be used to design a monitoring plan or strategy in a near-surface environment for geological carbon sequestration.« less

When CO 2 is injected in saline aquifers, dissolution causes a local increase in brine density that can cause Rayleigh-Taylor-type gravitational instabilities. Depending on the Rayleigh number, density-driven flow may mix dissolved CO 2 throughout the aquifer at fast advective time-scales through convective mixing. Heterogeneity can impact density-driven flow to different degrees. Zones with low effective vertical permeability may suppress fingering and reduce vertical spreading, while potentially increasing transverse mixing. In more complex heterogeneity, arising from the spatial organization of sedimentary facies, finger propagation is reduced in low permeability facies, but may be enhanced through more permeable facies. The connectivitymore » of facies is critical in determining the large-scale transport of CO 2-rich brine. We perform high-resolution finite element simulations of advection-diffusion transport of CO 2 with a focus on facies-based bimodal heterogeneity. Permeability fields are generated by a Markov Chain approach, which represent facies architecture by commonly observed characteristics such as volume fractions. CO 2 dissolution and phase behavior are modeled with the cubic-plus-association equation-of-state. Our results show that the organization of high-permeability facies and their connectivity control the dynamics of gravitationally unstable flow. Lastly, we discover new flow regimes in both homogeneous and heterogeneous media and present quantitative scaling relations for their temporal evolution.« less